High-entropy Doping Modification of High-nickel Single-crystal Layered Ternary Cathode Material

doi:10.15541/jim20250085

Abstract

Abstract:

LiNi_xCo_yMn_1-_x_-_yO₂ (NCM, x≥0.8), a promising cathode material for lithium-ion batteries, possesses high energy density and excellent discharge performance. However, it also appears drawbacks such as severe cation disorder, poor cycling performance and insecurity at high temperatures and high cut-off voltages. In this study, a high-entropy (HE) doping modification strategy was introduced into a high-nickel and low-cobalt LiNi_0.86Co_0.04Mn_0.1O₂ cathode material, and a high-nickel single-crystal layered ternary cathode material was synthesized by a high-temperature solid-state reaction method. The results show that at 0.1C (1C=180 mA·g^-1) and 25 ℃, the battery equipped with modified material has a reversible discharge capacity of 197 mAh·g^-1 and exhibits excellent discharge performance at high temperatures and high cut-off voltages. At 0.5C, 55 ℃ and 4.3 V, the discharge capacity reaches 281 mAh·g^-1, while at 0.5C, 25 ℃ and 4.5 V, the discharge capacity is as high as 194 mAh·g^-1. This material has a good layered structure with a uniform arrangement of nanoscale primary particles at microscale and a smaller total impedance. This work significantly improves cycling performance and safety of high-nickel ternary cathode materials at high temperatures and high cut-off voltages, providing a good modification method for the cobalt-free, high-nickel and practical application of ternary materials.

Key words: high-entropy, single crystal, high nickel and low cobalt, ternary cathode material

CLC Number:

O646

HOU Jiabing, HU Qiang, CUI Jiuzhi, HUANG Yundi, WANG Xinrui, LIU Xingquan. High-entropy Doping Modification of High-nickel Single-crystal Layered Ternary Cathode Material[J]. Journal of Inorganic Materials, 2026, 41(2): 193-200.

Figures/Tables 7

Fig. 1 XRD patterns of HE-NCM-sc and LE-NCM-sc (b) (003); (c) (006)/(012); (d) (018)/(110)

Fig. 2 SEM images of (a) precursor and (b) HE-NCM-sc

Fig. 3 SEM image and EDS elemental mappings of HE-NCM-sc

Fig. 4 In-depth XPS etching spectra of HE-NCM-sc

Fig. 5 (a) STEM, (b) TEM, and (c) HRTEM images of HE-NCM-sc

Fig. 6 Electrochemical performance of HE-NCM-sc and LE-NCM-sc cells (a) Rate performance; (b) Cycling performance at 0.1C; (c) Initial charging and discharging curves at 0.1C; (d) Cycling performance at 0.5C within the voltage range of 2.8−4.5 V; (e) Cycling performance at 0.5C and 55 ℃; (f) EIS spectra

Fig. 7 CV curve of HE-NCM-sc

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